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The Municipal Library is housed on the ground floor of the Cultural Center in the heart of Syros. Visitors of the library will find a rare and valuable collection of 45,000 volumes of literary publications and books.

The first official report of the library's operation states that in 1926, it housed around 2,000 volumes extracted from the literary collections from the library of the High School (1835) and in particular, from the library of Iakovos Rotas of the Bishop Anthimos Komnenos, who was a dear and beloved friend of Greek philosopher Adamantios Korais.

There is a particularly special place in the library which preserves old, delicate and precious books such as, but not limited to, Apollonius of Rhodium's "Argonautica" (1521), Rakinas' "Polucis Onomastikon" (1608), and Prince Rodokanakis' "Ioustinianai" (one of Syros' rare editions).